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Conical intersections serve as critical gateways in photochemical reactions, enabling rapid nonradiative transitions between potential energy surfaces that underpin fundamental processes such as photosynthesis or vision. Their calculation…

化学物理 · 物理学 2025-02-19 Rhyan Barrett , Christoph Ortner , Julia Westermayr

The conversion of photon energy into other energetic forms in molecules is accompanied by charge moving on ultrafast timescales. We directly observe the charge motion at a specific site in an electronically excited molecule using…

Electronically excited states of molecules are at the heart of photochemistry, photophysics, as well as photobiology and also play a role in material science. Their theoretical description requires highly accurate quantum chemical…

化学物理 · 物理学 2021-03-15 Julia Westermayr , Philipp Marquetand

We present a computationally efficient framework for predicting the excited-state properties of thermally activated delayed fluorescence (TADF) emitters, integrating extended tight-binding (\xtb), simplified Tamm-Dancoff approximation…

The description of excited state dynamics in multichromophoric systems constitutes both a theoretical and experimental challenge in modern physical chemistry. An experimental protocol which can systematically characterize both coherent and…

量子物理 · 物理学 2011-10-31 Joel Yuen-Zhou , Jacob J. Krich , Masoud Mohseni , Alán Aspuru-Guzik

A set formed by five reversibly-switchable fluorescent proteins (RSFPs) display spread over 40~nm in absorption maxima and only 18~nm in emission. The five proteins -- Dronpa, rsFastLime, rsKame, Padron(anionic form) and bsDronpa -- carry…

化学物理 · 物理学 2017-09-21 Daryna Smyrnova , María del Carmen Marín , Massimo Olivucci , Arnout Ceulemans

The development of X-ray free-electron lasers (XFELs) has enabled ultrafast X-ray diffraction (XRD) experiments, which are capable of resolving electronic/vibrational transitions and structural changes in molecules, or capturing molecular…

化学物理 · 物理学 2024-08-29 Sebastian V. Pios , Jiaji Zhang , Maxim F. Gelin , Hong-Guang Duan , Lipeng Chen

The ground and excited state calculations at key geometries, such as the Frank-Condon (FC) and the conical intersection (CI) geometries, are essential for understanding photophysical properties. To compute these geometries on noisy…

量子物理 · 物理学 2023-01-02 Shigeki Gocho , Hajime Nakamura , Shu Kanno , Qi Gao , Takao Kobayashi , Taichi Inagaki , Miho Hatanaka

We propose an excited-state molecular dynamics simulation method based on variational quantum algorithms at a computational cost comparable to that of ground-state simulations. We utilize the feature that excited states can be obtained as…

化学物理 · 物理学 2023-03-02 Hirotoshi Hirai

The accurate quantum chemical calculation of excited states is a challenging task, often requiring computationally demanding methods. When entire ground and excited potential energy surfaces (PESs) are desired, e.g., to predict the…

化学物理 · 物理学 2025-03-26 Zeno Schätzle , P. Bernát Szabó , Alice Cuzzocrea , Frank Noé

Effective photoinduced charge transfer makes molecular bimetallic assemblies attractive for applications as active light induced proton reduction systems. For a more sustainable future, development of competitive base metal dyads is…

The excited state dynamics of chromophores in complex environments determine a range of vital biological and energy capture processes. Time-resolved, multidimensional optical spectroscopies provide a key tool to investigate these processes.…

Multi-molecular excited states accompanied by an intra- and inter-molecular geometric relaxation are commonly encountered in optical and electrooptical studies and applications of organic semiconductors as, for example excimers or charge…

Photoactive iridium complexes are of broad interest due to their applications ranging from lighting to photocatalysis. However, the excited state property prediction of these complexes challenges ab initio methods such as time-dependent…

化学物理 · 物理学 2022-09-20 Gianmarco Terrones , Chenru Duan , Aditya Nandy , Heather J. Kulik

Light-induced chemical processes are ubiquitous in nature and have widespread technological applications. For example, photoisomerization can allow a drug with a photo-switchable scaffold such as azobenzene to be activated with light. In…

化学物理 · 物理学 2022-10-12 Simon Axelrod , Eugene Shakhnovich , Rafael Gómez-Bombarelli

A deep understanding of molecular photo-transformations is challenging because of the complex interaction between the configurations of electrons and nuclei. An initial optical excitation dissipates energy into electronic and structural…

Intersystem crossings between singlet and triplet states represent a crucial relaxation pathway in photochemical processes. Herein, we probe the intersystem crossing in hexafluoro-acetylacetone with ultrafast X-ray transient absorption…

We introduce a novel computational framework for excited-states molecular quantum dynamics simulations driven by quantum computing-based electronic-structure calculations. This framework leverages the fewest-switches surface-hopping method…

量子物理 · 物理学 2024-02-26 Anthony Gandon , Alberto Baiardi , Pauline Ollitrault , Ivano Tavernelli

Understanding the dynamic nature of protein structures is essential for comprehending their biological functions. While significant progress has been made in predicting static folded structures, modeling protein motions on microsecond to…

In this work, we extend the x-ray constrained wavefunction fitting approach, a key method in quantum crystallography for charge density reconstruction, to incorporate experimental observables beyond x-ray diffraction. Unlike traditional…

量子物理 · 物理学 2024-10-31 Stasis Chuchurka , Milaim Kas , Andrei Benediktovitch , Nina Rohringer
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